Angew.Chem.南昌大学徐香兰/王翔:亲氧Ru-O-Mn²⁺界面实现超高活性低温CO₂甲烷化

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Catalytic CO₂ methanation using renewable H₂ presents a promising strategy for carbon neutrality and renewable energy storage, yet achieving high efficiency at low temperatures remains a formidable challenge. Herein, we report a Ru/MnO catalyst featuring in situ constructed highly oxyphilic Ru-O-Mn²⁺ interfaces that demonstrate remarkable CO₂ methanation performance. At 180 ℃and a space velocity of 36,000 mLg⁻¹h⁻¹, the catalyst achieves 94.9% CO₂ conversion with a CH₄production rate of 84.7 µmolg_cat⁻¹s⁻¹, surpassing state-of-the-art catalysts, while maintaining robust stability. Combined experimental and theoretical investigations identify the Ru-O-Mn²⁺ interface as the pivotal active center, revealing a direct positive correlation between the amount of interfacial oxyphilic species, the quantity of weakly adsorbed CO₂, and the turnover frequency. This oxyphilic interfacial site establishes an extensive network for weak CO₂ adsorption, thereby promoting CO₂ activation at low temperatures. The successful extension of this strategy to Ni-based systems underscores the universality of MnO-mediated interfacial engineering. These findings establish a new design paradigm for low-temperature catalysis and deepen the fundamental understanding of interfacial oxyphilicity in heterogeneous catalysis.

要点1. 本文报道了一种Ru/MnO催化剂，其具有原位构筑的高亲氧性Ru-O-Mn²⁺界面，并展现出优异的二氧化碳甲烷化性能。在180℃和36,000 mLg⁻¹h⁻¹的空速下，该催化剂实现了94.9%的CO₂转化率，CH₄产率达到84.7 µmolg_cat⁻¹s⁻¹，超越了当前最先进的催化剂，同时保持了优异的稳定性。

要点2. 结合实验与理论研究发现，Ru-O-Mn²⁺界面是关键的活性中心，揭示了界面亲氧物种的数量、弱吸附CO₂的量与转换频率之间存在直接的正相关关系。这种亲氧性界面位点构建了一个广泛的弱CO2吸附网络，从而促进了CO₂在低温下的活化。该策略在Ni基体系中的成功应用，进一步印证了MnO介导的界面工程具有普适性。

要点3. 本文的研究发现为低温催化确立了一种新的设计范式，并加深了对多相催化中界面亲氧性的基本理解。

Shaorong Deng,Xiaowei Wang, Xiuzhong Fang, Xiang Wang*, Xianglan Xu*. Oxyphilic Ru-O-Mn²⁺ Interfaces on Ru/MnO Catalysts: Unprecedented Activity for Low-Temperature CO₂ Methanation. Angew. Chem. Int. Ed. 2026 , e6087744.

DOI: 10.1002/anie.6087744

https://doi.org/10.1002/anie.6087744

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